WO2014161877A1 - Procédé pour le co-traitement anaérobie d'eau contaminée par du cyanure et d'eau résiduaire comprenant de la matière organique fermentescible - Google Patents

Procédé pour le co-traitement anaérobie d'eau contaminée par du cyanure et d'eau résiduaire comprenant de la matière organique fermentescible Download PDF

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WO2014161877A1
WO2014161877A1 PCT/EP2014/056583 EP2014056583W WO2014161877A1 WO 2014161877 A1 WO2014161877 A1 WO 2014161877A1 EP 2014056583 W EP2014056583 W EP 2014056583W WO 2014161877 A1 WO2014161877 A1 WO 2014161877A1
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cyanide
anaerobic
reactor
solution
waste water
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PCT/EP2014/056583
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English (en)
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Blaz STRES
Doman NOVAK
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Universtiy Of Ljubljana
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    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F3/00—Biological treatment of water, waste water, or sewage
    • C02F3/28—Anaerobic digestion processes
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2101/00—Nature of the contaminant
    • C02F2101/10—Inorganic compounds
    • C02F2101/16—Nitrogen compounds, e.g. ammonia
    • C02F2101/18—Cyanides
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2101/00—Nature of the contaminant
    • C02F2101/30—Organic compounds
    • C02F2101/34—Organic compounds containing oxygen
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2103/00—Nature of the water, waste water, sewage or sludge to be treated
    • C02F2103/10—Nature of the water, waste water, sewage or sludge to be treated from quarries or from mining activities
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2103/00—Nature of the water, waste water, sewage or sludge to be treated
    • C02F2103/26—Nature of the water, waste water, sewage or sludge to be treated from the processing of plants or parts thereof
    • C02F2103/28—Nature of the water, waste water, sewage or sludge to be treated from the processing of plants or parts thereof from the paper or cellulose industry
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2103/00—Nature of the water, waste water, sewage or sludge to be treated
    • C02F2103/32—Nature of the water, waste water, sewage or sludge to be treated from the food or foodstuff industry, e.g. brewery waste waters
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2103/00—Nature of the water, waste water, sewage or sludge to be treated
    • C02F2103/32—Nature of the water, waste water, sewage or sludge to be treated from the food or foodstuff industry, e.g. brewery waste waters
    • C02F2103/327—Nature of the water, waste water, sewage or sludge to be treated from the food or foodstuff industry, e.g. brewery waste waters from processes relating to the production of dairy products
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2103/00—Nature of the water, waste water, sewage or sludge to be treated
    • C02F2103/34—Nature of the water, waste water, sewage or sludge to be treated from industrial activities not provided for in groups C02F2103/12 - C02F2103/32
    • C02F2103/343—Nature of the water, waste water, sewage or sludge to be treated from industrial activities not provided for in groups C02F2103/12 - C02F2103/32 from the pharmaceutical industry, e.g. containing antibiotics
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F3/00—Biological treatment of water, waste water, or sewage
    • C02F3/28—Anaerobic digestion processes
    • C02F3/2813—Anaerobic digestion processes using anaerobic contact processes
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F3/00—Biological treatment of water, waste water, or sewage
    • C02F3/28—Anaerobic digestion processes
    • C02F3/2833—Anaerobic digestion processes using fluidized bed reactors
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F3/00—Biological treatment of water, waste water, or sewage
    • C02F3/28—Anaerobic digestion processes
    • C02F3/2846—Anaerobic digestion processes using upflow anaerobic sludge blanket [UASB] reactors

Definitions

  • the topic of the invention is a procedure for anaerobic biological treatment of cyanide and production of biogas from cyanide using a mixture of cyanide contaminated industrial wastes and organic matter rich industrial wastes as inflow for the treatment in typical anaerobic biogas production reactors.
  • the procedure is based on anaerobic degradation of cyanide by microbial communities normally present in biogas production facilities, where the inflow to the reactor is a organic carbon rich wastewater amended with cyanide contaminated industrial wastewater, combining thus cyanide contaminated waste and organic carbon rich waste waters that normally originate from two different industrial sources.
  • Cyanide is commonly found as a contaminant in wastewaters from metal finishing industries, gold mining, pharmaceuticals and the food industry.
  • Industrial effluents generally contain between 0.01 and 10 mg ⁇ 1 of total cyanide; cyanide concentrations in natural systems are 100 ⁇ 500 times lower and range from 0.0001-0.05 mg ⁇ 1 (Wild et al., 1994). It is estimated that cyanide effluents from the industry can comprise up to approximately 14 million kg y 1 worldwide (ATSDR 2006).
  • the majority of cyanide waste waters are treated by chemical and physical treatments which are predominantly aerobic and often expensive and complex to operate (Dzombak et al 1996, Akcil 2003, Botz et al. 2005).
  • the hydrolytic pathway can be catalysed by five different microbial enzymes: (i) cyanide hydratase, (ii) nitriie hydratase, (iii) thiocyanate hydrolase, (iv) nitrilase, and (v) cyanidase.
  • the first three enzymes use cyanide as a substrate and directly hydrolyse and cleave the carbon-nitrogen triple bond to form formamide.
  • the last two enzymes convert cyanide to ammonia and formic acid, which are further utilized by other microorganisms (Gupta et al., 2010).
  • cyanide removal can occur by abiotic hydrolysis of cyanide to formate as first reported by Sanchez et al. (1967).
  • Cyanide in various industrial wastewaters is resistant to anoxic microbial degradation due to low content or the quality of anaerobically degradable carbon.
  • the problem of organic carbon dependency for effective microbial removal of various contaminants in bacterostats was solved by addition of aqueous mixture of at least one carbohydrate and at least one alcohol (patent US7144509). Cyanide was at least partially removed, when added to conventional wastewater treatment plant (patent US8303849, WO2013005212), however, with the drawback of possible partial diffusion to gaseous phase.
  • the object of this invention is to detoxify cyanide contaminated waste waters and sludges, avoiding the expensive and toxic chemical or time-consuming and incomplete (micro) erobic plant-fungi (or other) mediated procedures of the prior art thus shortening the time needed for cyanide degradation and increasing the control over cyanide leakage into soils/waters/air during its degradation.
  • a method for anaerobic degradation of cyanide comprising: a) providing a solution comprising cyanide and fermentable organic matter having a chemical oxygen demand (COD) of 1500-12,000 mg/1; and b) treating the solution in an anaerobic digestion reactor.
  • COD chemical oxygen demand
  • the solution in step a) is provided by mixing a first solution of cyanide containing industrial waste water with a second solution comprising the fermentable organic matter.
  • mixing is in continuous mode or in batch mode.
  • the cyanide concentration in the solution is 0.01 -10 mg/1, more preferably 0.0001- 10 me/1.
  • the second solution comprising the fermentable organic matter is brewery waste water, dairy waste water, starch loaded water, corn loaded water, fructose syrup loaded water, spent non- and/or alcoholic beverages, effluent from sugar factories, effluent from paper mills, effluent from paper industries, or mixtures thereof, preferably brewery waste water.
  • the first solution of cyanide containing industrial waste water is finishing industry waste water, gold mining waste water, pharmaceutical industries waste water, or mixtures thereof.
  • Typical anaerobic bio-reactors to be used as the anaerobic digestion reactor including an upflow anaerobic sludge blanket-reactor (UASB-reactor), continuously stirred tank-reactor (CSTR-reactor), anaerobic contact process-reactor (ACP-reactor), upflow-downflow anaerobic filter reactor (U-DAF-reactor), fluidized bed-reactor (FB-reactor) treating waste by complex anaerobic microbial communities are described in details by Deublein and Steinhsuser (2008), Kaparaju et al. (2009), aksonen and Puhakka (2007), Lichtfouse (201 1) and others.
  • the anaerobic digestion reactor is an upflow anaerobic sludge blanket-reactor (UASB-reactor) or continuously stirred tank-reactor (CSTR-reactor) or anaerobic contact process-reactor (ACP-reactor) or upflow-downflow anaerobic filter reactor (U-DAF-reactor), fluidized bed-reactor (FB-reactor).
  • UASB-reactor upflow anaerobic sludge blanket-reactor
  • CSTR-reactor continuously stirred tank-reactor
  • ACP-reactor anaerobic contact process-reactor
  • U-DAF-reactor upflow-downflow anaerobic filter reactor
  • FB-reactor fluidized bed-reactor
  • the solution has a COD of 1500-9000 mg/1, preferably 2000-6000 mg/1.
  • the fermentable organic matter comprises pentose, hexose, disaccharides, oligosaccharides, polysaccharides, proteins or lipids.
  • the fermentable organic matter comprises molecules having keto- and/or aldehyde-group(s) .
  • the method is further comprising a pretreating step carried out after step a) and before step b) or before mixing, comprising reacting at least parts of the cyanide and the fermentable organic matter under abiotic conditions.
  • the concentration of the cyanide in the solution is more than 10 mg/1.
  • reacting comprises Cyanhydrine-Synthesis ( iliani-Fischer-Synthesis) reaction.
  • the task is solved with a procedure that enables the production of biogas with high methane content from cyanide in the typical anaerobic biogas production reactors.
  • the task is solved with a procedure of combining cyanide contaminated industrial waste waters, with low organic carbon content (e.g. finishing industries, gold mining, pharmaceuticals but not excluding other sources) in continuous or batch mode with specific industrial waste waters containing high fraction of fermentable dissolved organic carbon (e.g.
  • the reactors that receive cyanide for the first time can be operated in continuous mode with low cyanide concentrations (up to 1 mg / L) or sequentially using almost an order of magnitude higher cyanide concentrations (8.5 mg IV), using biomass without previous historical exposures or adaptation to cyanide.
  • the dissolved organic carbon is used in the form of various molecular types in the range of COD concentration between 1500 mg / L and 12000 mg /L, although the concentrations within the range of 2000 mg / L to 6000 mg / L are preferred, depending on the hydraulic retention time.
  • the dissolved organic carbon molecules should be pentoses, hexoses, di-oligo-polysaccharides next to proteins and lipids and also trace elements from various residual industrial sources, exhibiting mainly keto- and/or aldehide- functional groups. Two or more sources can be combined to achieve this. It was surprisingly found that the procedure according to the invention organic carbon provided by inflow of organic rich waters serves triple purpose when mixed with cyanide contaminated waters:
  • Wiley-VCH 443 pp.
  • Figure 1 Cumulative biogas production in anaerobic batch reactors amended with brewery waste water (BWW) and 5.0 or 8.5 mg ⁇ 1 of cyanide. Values are means of three replicates. SD is omitted for clarity.
  • FIG. 2 Methane content (A) and cumulative methane production (B) in anaerobic batch reactors amended with brewery waste water (BWW) and 5.0 or 8.5 mg ⁇ 1 of cyanide. Values are means of three replicates. SD is omitted for clarity.
  • FIG. 4 Concentrations of free cyanide in anaerobic batch reactors containing autoclaved or non-autoclaved brewery waste water (BWW) with 3.0 mg ⁇ 1 of cyanide during 14 days of incubation. Values are means of three replicates ⁇ SD.
  • FIG. 1 Comparison of T-RFLP profiles of bacterial (A) and archaeal (B) microbial communities present in UASB biomass after the incubation in the presence of cyanide.
  • TO - initial state Blank - endpoint UASB biomass; BWW -endpoint UASB biomass with brewe .' waste water (BWW); BWW+CN5 - endpoint BWW amended with 5.0 mg ⁇ 1 cyanide; BWW+CN8.5 - endpoint brewery waste water amended with 8.5 mg ⁇ 1 cyanide.
  • Figure 6 Canonical ordination of archaeal communities present in UASB biomass. labc- initial state; 2abc - developed blank; 3abc - developed BWW; 4abc - developed BWW amended with 5.0 mg ⁇ 1 cyanide ; 5abc - developed BWW amended with 8.5 mg ⁇ 1 cyanide.
  • the arrows indicate the increase in the gradient of signal intensity of the most important microarray probes significantly associated with the distribution of samples (Msarl97- ethanosarcina; MbM405-Methanobacterium and Methanothermobacter; Mspi422- Methanospirillum; Mbre377-Methanobrevibacter). See text for further explanation
  • the procedure of production of biogas with high methane content from cyanide in the typical anaerobic biogas production reactors occurs after combining cyanide contaminated industrial waste waters from finishing industries, gold mining, pharmaceuticals and the food industry by mixing or dillution with organic matter rich industrial waste waters containing high fraction of fermentable dissolved organic carbon (pentoses, hexoses, di-oligo-polysaccharides, aldehides, ketones next to proteins and lipids and also trace elements) from brewery and dairy waste waters, starch, corn, fructose syrup loaded waters, spent non- and alcoholic beverages, effluents from sugar factories, paper mills and industries, green chemistry synthesis reactions, algae ponds and photobioreactors containing algal and other biomass, molasses, in typical anaerobic digesters.
  • fermentable dissolved organic carbon pentoses, hexoses, di-oligo-polysaccharides, aldehides, ketones next to proteins and lipids and also trace elements
  • waste waters containing dissolved organic material ensures that the biomass responds to its addition, synthesizes the needed enzymes, breaks down cyanide into organic compounds that can be transformed into additional quantities of biogas while completely removing cyanide.
  • the dissolved organic carbon is used in the form of various molecular types in the range of COD concentration between 1500 mg / L and 9000 mg /L, although the concentrations within the range of 2000 mg / L to 6000 mg / L are preferred.
  • the use of mixing of two or more industrial waters containing cyanide and organic matter rich industrial waste waters ensures that the residing biomass responds to the substrate combination and can initiate cyanide degradation instantly degrading cyanide in concentrations above the inhibitory concentration and producing additional biogas and methane.
  • the biomass that is shock-loaded by cyanide is only temporarily inhibited.
  • the makings of suitable conditions to allow for Kiiiani-Fischer chemical reactions lowers the cyanide inhibitory concentration below the inhibitory threshold resulting in a pick-up of microbial activity and an increased production of biogas and methane from the reaction products.
  • the anaerobic biomass treating brewery waste water or other substrates is mixed with the cyanide containing waste waters enabling instant cyanide degradation or in the case of inhibition by too high cyanide concentration, a self-regulating chemical mechanism that lowers the cyanide barrier, allowing microorganisms to fully degrade cyanide and build their cyanide resistance.
  • EXAMPLE 1 The combination of brewery waste water and cyanide substrate for efficient anaerobic cyanide degradation and biogas production in anaerobic sludge blanket (UASB) reactor biomass.
  • the methanogenic activity of unadapted granulated biomass was detected at higher cyanide concentrations than reported previously for the unadapted suspended biomass, making the aggregated structure and predominantly hydrogenotrophic nature of methanogenic community important features in cyanide degradation.
  • the inoculum for anaerobic granulated biomass was obtained from an industrial UASB (upflow anaerobic sludge blanket) reactor.
  • the UASB reactor had been in operation for > 2 yr. treating brewery wastewaters (BWW) at a loading rate 4 g COD 3 _i day "1 . It was operated mesophilically at 37 °C and had a hydraulic retention time of 40 h.
  • a soluble organic carbon removal efficiency of >90 % was determined by the chemical oxygen demand (COD).
  • Total solids (TS) were 43.7 g I 4
  • the volatile solids (VS) were 48.4 % of TS.
  • COD, TS and VS were determined according to the APHA standard methods (APHA 2005).
  • Oxitop bottles 1000 ml equipped with pressure sensors (WTW, Germany) were used as anaerobic batch reactors. Side neck sampling ports were sealed with butyl rubber stoppers to prevent gas leakage. Reactors were inoculated with 40 ml of biomass from the UASB reactor. Samples were amended with 60 ml of brewery waste water (180 mg of COD as carbon source), 20 ml of phosphate buffer and diluted with deoxygenated water to 500 ml. Blank samples received no brewery waste water addition and served to monitor the basal metabolic activity.
  • the reactors were supplemented with KCN to obtain the following cyanide concentrations: 1 , 2, 3, 5 and 8.5 mg ⁇ 1 .
  • Total biogas produced during 60 days of incubation was measured hourly using pressure-sensor data loggers. Biogas measurements served as descriptors of the initial lag phases, the biogas production velocity and the total amount of biogas produced. Headspace gas composition was measured on days 0, 7, 14, 21 , 28, 35 and 60 by gas chromatograph coupled to mass spectrometer (GC-QMS analysis).
  • GC-QMS analysis gas chromatograph coupled to mass spectrometer
  • Methane content during the 60 days of incubation was comparable between the positive control and the samples amended with 5.0 mg 1-1 of cyanide, accounting for 80 % of biogas on average. In accordance with biogas production, a small amount of methane was detected in samples amended with 8.5 mg 1-1 of cyanide during the first two days of incubation.

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  • Life Sciences & Earth Sciences (AREA)
  • Microbiology (AREA)
  • Biodiversity & Conservation Biology (AREA)
  • Hydrology & Water Resources (AREA)
  • Engineering & Computer Science (AREA)
  • Environmental & Geological Engineering (AREA)
  • Water Supply & Treatment (AREA)
  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Purification Treatments By Anaerobic Or Anaerobic And Aerobic Bacteria Or Animals (AREA)

Abstract

La présente invention porte sur un procédé pour le traitement biologique anaérobie de cyanure et la production de biogaz à partir de cyanure à l'aide d'un mélange de rejets industriels contaminés par du cyanure et de rejets industriels riches en matière organique utilisés comme flux entrant pour le traitement dans des réacteurs typiques de production anaérobie de biogaz. Le procédé est basé sur la dégradation anaérobie de cyanure par des communautés microbiennes normalement présentes dans des installations de production de biogaz, le flux entrant dans le réacteur étant un mélange d'eau résiduaire industrielle contaminée par du cyanure et d'eau résiduaire riche en carbone organique de type particulier. Le procédé permet une dégradation instantanée du cyanure par des consortiums microbiens. Dans le cas d'une inhibition par du cyanure, les conditions du réacteur permettent également une réaction chimique de détoxification du cyanure qui abaisse efficacement la concentration en cyanure inhibitrice et permet la conversion à médiation microbienne de cyanure et de ses dérivés abiotiques en biogaz et méthane supplémentaires.
PCT/EP2014/056583 2013-04-03 2014-04-02 Procédé pour le co-traitement anaérobie d'eau contaminée par du cyanure et d'eau résiduaire comprenant de la matière organique fermentescible WO2014161877A1 (fr)

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SI201300086A SI24343A (sl) 2013-04-03 2013-04-03 Procedura za odstranjevanje cianida iz onesnaĹľenih vod in produkcija bioplina iz cianida
SI201300086 2013-04-03

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Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN107399877A (zh) * 2017-07-27 2017-11-28 郑州大学环境技术咨询工程有限公司 一种高浓度多组分有机废水的集成处理技术
CN109231671A (zh) * 2018-10-10 2019-01-18 常州方圆制药有限公司 一种多级厌氧处理硫酸依替米星生产废水的方法
CN110621772A (zh) * 2017-02-08 2019-12-27 生物保护公司 作为用于废水处理的添加剂的干燥微生物污泥颗粒
CN113772881A (zh) * 2021-08-28 2021-12-10 北京百灵天地环保科技股份有限公司 一种酚氰废水的氧化处理方法

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DE102005023598A1 (de) * 2005-05-18 2006-11-23 Technische Universität Braunschweig Carolo-Wilhelmina Verfahren zur Dekontamination von cyanidhaltigen Böden/Aquiferen und Grundwässer
WO2009059819A1 (fr) * 2007-11-09 2009-05-14 Upm-Kymmene Oyj Traitement des eaux usées issues d'un processus de transformation de la biomasse en liquide comprenant la production de gaz de synthèse et installations d'usine intégrées

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DE102005023598A1 (de) * 2005-05-18 2006-11-23 Technische Universität Braunschweig Carolo-Wilhelmina Verfahren zur Dekontamination von cyanidhaltigen Böden/Aquiferen und Grundwässer
WO2009059819A1 (fr) * 2007-11-09 2009-05-14 Upm-Kymmene Oyj Traitement des eaux usées issues d'un processus de transformation de la biomasse en liquide comprenant la production de gaz de synthèse et installations d'usine intégrées

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Title
ANNACHHATRE A P ET AL: "UPFLOW ANAEROBIC SLUDGE BLANKET TREATMENT OF STARCH WASTEWATER CONTAINING CYANIDE", RESEARCH JOURNAL OF THE WATER POLLUTION CONTROL FEDERATION, WATER POLLUTION CONTROL FEDERATION, ALEXANDRIA, VA, US, vol. 73, no. 5, 1 September 2001 (2001-09-01), pages 622 - 632, XP001124721, ISSN: 1047-7624 *

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN110621772A (zh) * 2017-02-08 2019-12-27 生物保护公司 作为用于废水处理的添加剂的干燥微生物污泥颗粒
CN107399877A (zh) * 2017-07-27 2017-11-28 郑州大学环境技术咨询工程有限公司 一种高浓度多组分有机废水的集成处理技术
CN109231671A (zh) * 2018-10-10 2019-01-18 常州方圆制药有限公司 一种多级厌氧处理硫酸依替米星生产废水的方法
CN113772881A (zh) * 2021-08-28 2021-12-10 北京百灵天地环保科技股份有限公司 一种酚氰废水的氧化处理方法

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